The resonant interaction of light with metal nanoparticles can result in extraordinary optical effects in both the near and far fields. Plasmonics, the study of this interaction, has the potential to enhance performance in a wide range of applications, including sensing, photovoltaics, photocatalysis, biomedical imaging, diagnostics, and treatment. However, the mechanisms of plasmonic enhancement often remain poorly understood, limiting the design and effectiveness of plasmonics for advanced applications. This dissertation focuses on evaluating the mechanisms of plasmonic enhancement and distinguishing between near and far field effects using simulations and experimental results. Thorough characterization of metal nanoparticle colloids shows that electromagnetic simulations can be used to accurately predict the optical response of nanoparticles only if the true shapes and size distributions are taken into account. By coupling these optical interaction calculations with heat transfer models, experimental limits for the maximum optical power before nanoparticle melting can be found. These limits are important for plasmonic multiphoton luminescence imaging applications. Subsequently, we demonstrate ultrafast laser plasmonic nanoablation of silicon substrates using gold nanorods to identify the near-field enhancement and mechanism of plasmon-assisted ablation. The experimentally observed shape of the ablation region and reduction of the ablation threshold are compared with simulations to show the importance of the enhanced electromagnetic fields in near-field nanoablation with plasmonic nanoparticles. The targeted use of plasmonic nanoparticles requires narrow size distribution colloids, because wide size distributions result in a blurring and weakening of the optical response. A new synthesis method is presented for the seeded-growth of nearly monodisperse metal nanoparticles ranging from 10 to 100 nm in diameter, both with and without dielectric shells of controlled thickness. This method is used to acquire fine control over the position and width of the plasmonic peak response. We also demonstrate self-assembled sub-monolayers of these particles with controllable concentrations, which is ideal for looking at plasmonic effects in surface and layered geometries. Finally, we present results for the spatial distribution of absorption around plasmonic nanoparticles. We introduce field-based definitions for distinguishing near-field and far-field regions and develop a new set of equations to determine the point-by-point enhanced absorption in a medium around a plasmonic nanoparticle. This set of equations is used to study plasmon-enhanced optical absorption for thin-film photovoltaic cells. Plasmonic nanoparticle systems are identified using simulations and proof-of-concept experiments are used to demonstrate the potential of this approach.

The resonant interaction of light with metal nanoparticles can result in extraordinary optical effects in both the near and far fields. Plasmonics, the study of this interaction, has the potential to enhance performance in a wide range of applications, including sensing, photovoltaics, photocatalysis, biomedical imaging, diagnostics, and treatment. However, the mechanisms of plasmonic enhancement often remain poorly understood, limiting the design and effectiveness of plasmonics for advanced applications. This dissertation focuses on evaluating the mechanisms of plasmonic enhancement and distinguishing between near and far field effects using simulations and experimental results. Thorough characterization of metal nanoparticle colloids shows that electromagnetic simulations can be used to accurately predict the optical response of nanoparticles only if the true shapes and size distributions are taken into account. By coupling these optical interaction calculations with heat transfer models, experimental limits for the maximum optical power before nanoparticle melting can be found. These limits are important for plasmonic multiphoton luminescence imaging applications. Subsequently, we demonstrate ultrafast laser plasmonic nanoablation of silicon substrates using gold nanorods to identify the near-field enhancement and mechanism of plasmon-assisted ablation. The experimentally observed shape of the ablation region and reduction of the ablation threshold are compared with simulations to show the importance of the enhanced electromagnetic fields in near-field nanoablation with plasmonic nanoparticles. The targeted use of plasmonic nanoparticles requires narrow size distribution colloids, because wide size distributions result in a blurring and weakening of the optical response. A new synthesis method is presented for the seeded-growth of nearly monodisperse metal nanoparticles ranging from 10 to 100 nm in diameter, both with and without dielectric shells of controlled thickness. This method is used to acquire fine control over the position and width of the plasmonic peak response. We also demonstrate self-assembled sub-monolayers of these particles with controllable concentrations, which is ideal for looking at plasmonic effects in surface and layered geometries. Finally, we present results for the spatial distribution of absorption around plasmonic nanoparticles. We introduce field-based definitions for distinguishing near-field and far-field regions and develop a new set of equations to determine the point-by-point enhanced absorption in a medium around a plasmonic nanoparticle. This set of equations is used to study plasmon-enhanced optical absorption for thin-film photovoltaic cells. Plasmonic nanoparticle systems are identified using simulations and proof-of-concept experiments are used to demonstrate the potential of this approach. / text

Plasmonic Laser Nanosurgery (PLN) is a novel photodisruption technique that exploits the large enhancement of ultrafast laser pulses in the near-field of gold nanoparticles for the nanoscale manipulation of biological structures. Excitation of surface plasmons on spherical nanoparticles by pulsed irradiation provides a platform for the confinement of photoactivated processes, while functionalized nanoparticle targeting methods provide the highest level of therapeutic selectivity. In this dissertation, we demonstrate and characterize the in vitro plasmonic optoporation of MDA-MB-468 human epithelial breast cancer cells labeled with plasmonic gold nanoparticles using NIR, femtosecond laser pulses. Using a 10 kDa FITC-Dextran probe dye, we find that the PLN can optoporate nanoparticle-labeled cellular membranes at fluences down to just a few mJ/cm², providing a 50-fold reduction in pulse energy necessary to induce membrane dysfunction as compared with unlabeled cells. Limited membrane dysfunction was found to lead to transient optoporation of cells as a possible transfection method, while more extensive, non-recoverable membrane dysfunction lead to cellular death as a possible plasmonic treatment of malicious cells. In the first regime, we found a maximum optoporation efficiency of approximately 31% ± 5.4% with 2 to 2.5 mW laser light having 80 MHz repetition rate. In the second regime, we were able to necrotically kill greater than 90% of irradiated cells with as little as 5 mW average power. We found that particle aggregation along the cellular surface is crucial for the success of PLN. High particle loadings were required, suggesting that particle aggregates provide large enhancements, leading to reduced PLN threshold energies. We provide experimental evidence suggesting photodisruption with ultra-low energy pulses is directly dependent upon the emission of electrons from the particle surface, which seed the formation of free radicals in the surrounding water. These free radicals mediate membrane dysfunction by polyunsaturated lipid and protein peroxidation. / text

This thesis reports on the work performed on the manipulation of micro­-particles on substrate surfaces using short laser pulses. For particles with diameters on the order of microns, the binding forces to surfaces are significantly larger than gravitational forces. To overcome these binding forces and manipulate the particles the use of femtosecond laser pulses has been investigated. Individual micro-particles (poly-divinylbenzene, glass and silver materials) with diameters around 2 um were removed from substrate surfaces (dielectric, semiconductor and metal substrates) us­ing a Ti:Sapphire laser system. The pulses produced at 800 nm had pulse lengths around 140 fs and were tightly focussed onto the surface using 5x and 10x micro­scope objectives. The peak fluence thresholds for particle removal were determined and the surfaces examined after irradiation by a scanning electron microscope and atomic force microscope to check for damage. The experimental results indicate that ablation of the substrate below the micro-particles is most likely to be respon­sible for micro-particle removal from the substrate surface when using femtosecond pulses. Ablation pits were observed for the dielectric micro-spheres on semiconductor substrates. It is also believed that ablation is responsible for the removal of other types of micro-particles from various substrates. Unlike the dielectric micro-sphere on semiconductor substrate results, the other particle-substrate combinations show a close correspondence between the removal and substrate ablation thresholds. It is believed that these results indicate the occurrence of ablation leading to the removal of the micro-particles. Calculations of the local electromagnetic fields around the micro-particles have also been carried out and the distributions used to interpret the experimental results. / Thesis / Master of Applied Science (MASc)

Attosecond pulses have been developed as a means for investigating phenomena that proceed on the order of the atomic unit of time (24 as). Unfortunately, these extreme ultraviolet (XUV) pulses by themselves contain too few photons to initiate nonlinear dynamics or dress states in an attosecond pump--attosecond probe scheme. As a result, most attosecond experiments thus far have featured complementary near infrared (NIR) femtosecond lasers for instigating electron dynamics. In order to access the benefits of all-attosecond measurements and open attosecond physics to new fields of exploration, the photon flux of these pulses must be increased. One way to boost the attosecond pulse energy is to scale up the energy of the NIR pulse responsible for driving high-harmonic generation (HHG). With generalized double optical gating (GDOG), isolated attosecond pulses can be generated with multi-cycle laser systems, wherein the pulse energy can be boosted more easily than in the few-cycle laser systems required by other gating methods. At the Institute for the Frontier of Attosecond Science and Technology (IFAST), this scalability was demonstrated using a 350 mJ, 15 fs (10 TW) Ti:sapphire laser, which was used to generate a 100 nJ XUV continuum. This represented an order-of-magnitude improvement over typical attosecond pulse energies achievable by millijoule-level few-cycle lasers. To obtain the microjoule-level attosecond pulse energy required for performing all-attosecond experiments, the attosecond flux generated by the IFAST 10 TW system was still deficient by an order of magnitude. To this end, the laser system was upgraded to provide joule-level output energies while maintaining pulse compression to 15 fs, with a targeted peak power of 200 TW. This was accomplished by adding an additional Ti:sapphire amplifier to the existing 10 TW system and implementing a new pulse compression system to accommodate the higher pulse energy. Because this system operated at a 10 Hz repetition rate, stabilization of the carrier-envelope phase (CEP) -- important for controlling attosecond pulse production -- could not be achieved using traditional methods. Therefore, a new scheme was developed, demonstrating the first-ever control of CEP in a chirped-pulse amplifier (CPA) at low repetition rates. Finally, a new variation of optical gating was proposed as a way to improve the efficiency of the attosecond pulse generation process. This method was also predicted to allow for the generation of isolated attosecond pulses with longer driving laser pulses, as well as the extension of the high-energy photon cut-off of the XUV continuum.

Master of Science / Department of Physics / Itzhak Ben-Itzhak / Imaging the interaction of molecular ion beams with ultrafast intense laser fields is a very powerful method to understand the fragmentation dynamics of molecules. Femtosecond laser pulses with different wavelengths and intensities are applied to dissociate and ionize molecular ions, and each resulting fragmentation channel can be studied separately by implementing a coincidence three-dimensional (3D) momentum imaging method. The work presented in this master’s report can be separated into two parts. First, the interaction between molecular ion beams and femtosecond laser pulses, in particular, the dissociation of CO[superscript]+ into C[superscript]++O, is studied. For that purpose, measurements are conducted at different laser intensities and wavelengths to investigate the possible pathways of dissociation into C[superscript]++O. The study reveals that CO[superscript]+ starts to dissociate from the quartet electronic state at low laser intensities. Higher laser intensity measurements, in which a larger number of photons can be absorbed by the molecule, show that the doublet electronic states with deeper potential wells, e.g. A [superscript]2Π, contribute to the dissociation of the molecule. In addition, the three-body fragmentation of CO[subscript]2[superscript]+ into C[superscript]++O[superscript]++O[superscript]+ is studied, and two breakup scenarios are separated using the angle between the sum and difference of the momentum vectors of two O[superscript]+ fragments. In the second part, improvements in experimental techniques are discussed. Development of a reflective telescope setup intended to increase the conversion efficiency of ultraviolet (UV) laser pulse generation is described, and the setup is used in the studies of CO[superscript]+ dissociation described in this report. The other technical study presented here is the measurement of the position dependence of timing signals picked off of a microchannel plate (MCP) surface. The experimental method is presented and significant time spread over the surface of the MCP detector is reported [1].

Šios disertacijos tikslas – didelio tikslumo matuoklio, skirto šiluminio lęšio lazerių aktyviuosiuose elementuose matavimams sukūrimas, bei įvairių metodų, skirtų šiluminio lęšio įtakos mažinimui tyrimas. Matavimai buvo atliekami Shack‘o ir Hartmann‘o bangos fronto matuokliu, kuris buvo pritaikytas mažų skersinių matmenų (<1x1 mm) šiluminio lęšio matavimams. Pademonstruotas naujos konstrukcijos asferinis kompensatorius iš esmes mažinantis šiluminio lęšio aberacijų įtaką išilginio diodinio kaupinimo lazeriuose. Atlikti šiluminio lęšio aberacijų matavimai buvo panaudoti kompensatoriaus profilio skaičiavimams. Naudojant asferinį kompensatorių, pagamintą plonasienių dangų užgarinimo būdu, generacijos slenkstis sumažėjo daugiau kaip 3 kartus, taip pat ženkliai pagerėjo lazerio pluošto intensyvumo skirstinys. Darbe nagrinėjamas stiprinamų impulsų energijos didinimo būdas pasitelkiant eliptinę rezonatoriaus modą Yb:IAG lazeryje. Šis metodas leidžia kelis kartus padidinti stiprinamų impulsų energiją, išlaikant dirakciškai ribotus erdvinius pluošto parametrus. Taip pat, surasta lazerio rezonatoriaus konfigūracija, leidžianti palaikyti stipriai astigmatišką modą aktyviajame elemente, ir simetrišką modą lazerio išėjime. Pateikiami šiluminio lęšio matavimų rezultatai „atermalinės“ ir Ng orientacijos Yb:KGW kristaluose. Taip pat, parodėme, kad kristalo galų išsigaubimo įtaka Ng orientacijos Yb:KGW aktyviuosiuose elementuose gali siekti 50%. Atlikti tyrimai parodė, kad išbandyta... [toliau žr. visą tekstą] / In this thesis, analysis of thermal effects and various approaches for their mitigation in diode end pumped ultrafast lasers is presented. Experimental investigations were performed by employing Shack-Hartmann wavefront sensor which was adapted for measurements of thermal lens in diode end pumped lasers. During research, operation of high average power, diode-pumped, Nd:YVO4 laser with aspheric aberration corrector was investigated. Actual thermal lens measurements were conducted in order to design properly shaped aberration corrector that was manufactured using a thin film deposition technology. This allows us to conclude that employment of proper thermal lens aberration compensator allowed for laser threshold reducing and ensured improved output beam quality parameter M2 in wide pump power range. Prospects of output pulse energy scaling in diode end-pumped Yb:YAG laser by employing elliptical mode geometry was investigated. During our experiments, maximum average power in of ~ 5.5 W was obtained at repetition rates of 30-100 kHz, while in CW operation mode the 8 W output power was achieved. In spite of strongly astigmatic thermal lens due to optimized cavity design the output beam exhibits high spatial quality: beam quality parameter M2 in both vertical and horizontal plane was close to unity. Detailed comparative study of thermal effects in Yb doped KGW crystals with different orientation was performed. Measurements confirm, that anisotropic optical and thermal properties... [to full text]

In this thesis, analysis of thermal effects and various approaches for their mitigation in diode end pumped ultrafast lasers is presented. Experimental investigations were performed by employing Shack-Hartmann wavefront sensor which was adapted for measurements of thermal lens in diode end pumped lasers. During research, operation of high average power, diode-pumped, Nd:YVO4 laser with aspheric aberration corrector was investigated. Actual thermal lens measurements were conducted in order to design properly shaped aberration corrector that was manufactured using a thin film deposition technology. This allows us to conclude that employment of proper thermal lens aberration compensator allowed for laser threshold reducing and ensured improved output beam quality parameter M2 in wide pump power range. Prospects of output pulse energy scaling in diode end-pumped Yb:YAG laser by employing elliptical mode geometry was investigated. During our experiments, maximum average power in of ~ 5.5 W was obtained at repetition rates of 30-100 kHz, while in CW operation mode the 8 W output power was achieved. In spite of strongly astigmatic thermal lens due to optimized cavity design the output beam exhibits high spatial quality: beam quality parameter M2 in both vertical and horizontal plane was close to unity. Detailed comparative study of thermal effects in Yb doped KGW crystals with different orientation was performed. Measurements confirm, that anisotropic optical and thermal properties... [to full text] / Šios disertacijos tikslas – didelio tikslumo matuoklio, skirto šiluminio lęšio lazerių aktyviuosiuose elementuose matavimams sukūrimas, bei įvairių metodų, skirtų šiluminio lęšio įtakos mažinimui tyrimas. Matavimai buvo atliekami Shack‘o ir Hartmann‘o bangos fronto matuokliu, kuris buvo pritaikytas mažų skersinių matmenų (<1x1 mm) šiluminio lęšio matavimams. Pademonstruotas naujos konstrukcijos asferinis kompensatorius iš esmes mažinantis šiluminio lęšio aberacijų įtaką išilginio diodinio kaupinimo lazeriuose. Atlikti šiluminio lęšio aberacijų matavimai buvo panaudoti kompensatoriaus profilio skaičiavimams. Naudojant asferinį kompensatorių, pagamintą plonasienių dangų užgarinimo būdu, generacijos slenkstis sumažėjo daugiau kaip 3 kartus, taip pat ženkliai pagerėjo lazerio pluošto intensyvumo skirstinys. Darbe nagrinėjamas stiprinamų impulsų energijos didinimo būdas pasitelkiant eliptinę rezonatoriaus modą Yb:IAG lazeryje. Šis metodas leidžia kelis kartus padidinti stiprinamų impulsų energiją, išlaikant dirakciškai ribotus erdvinius pluošto parametrus. Taip pat, surasta lazerio rezonatoriaus konfigūracija, leidžianti palaikyti stipriai astigmatišką modą aktyviajame elemente, ir simetrišką modą lazerio išėjime. Pateikiami šiluminio lęšio matavimų rezultatai „atermalinės“ ir Ng orientacijos Yb:KGW kristaluose. Taip pat, parodėme, kad kristalo galų išsigaubimo įtaka Ng orientacijos Yb:KGW aktyviuosiuose elementuose gali siekti 50%. Atlikti tyrimai parodė, kad išbandyta... [toliau žr. visą tekstą]

Methods of controlling molecular rotations using linearly polarized femtosecond and picosecond pulses are considered and analyzed theoretically. These laser pulses, typically in the infrared, are highly non-resonant with respect to the electronic degrees of freedom of the molecules and have intensities of &sim; 10^13 to 10^14 W/cm&sup2;. It is shown how these laser pulses can force small linear molecules to align with the direction of the electric field vector of the laser both in the presence of the laser field as well as after the application of a short laser pulse. Recent experiments on laser-induced molecular alignment are modeled and excellent agreement between experiment and theory is found. Additional methods of controlling molecular rotational dynamics are outlined. The first method considers the forced rotational acceleration of diatomic molecules, called the <i>optical centrifuge</i>. Here, the direction of polarization of a linearly polarized laser field is made to smoothly rotate faster and faster. The molecules, which tend to align with the polarization vector of the laser field, follow the rotation of the laser polarization and are accelerated to high angular momentum. The second method considers the control of field-free rotational dynamics by applying phase shifts to the molecular wave function at select times called <i>fractional revivals</i>. At these select moments, an initially localized wave function splits into several copies of the initial state. Adding phase shifts to the copies then induces interference effects which can be used to control the subsequent evolution of the rotational wave function. This same control scheme has a close link to quantum information and this connection is outlined. Finally, a recently proposed method of controlling the quantum dynamics of the classically chaotic kicked rotor system [J. Gong and P. Brumer, Phys. Rev. Lett. 86, 1741 (2001)] is analyzed from a phase space perspective. It is shown that the proposed quantum control can be linked to small islands of stability in the classical phase space. An experimentally feasible variant of this control scenario using wave packets of molecular alignment is proposed. Two applications of molecular alignment are discussed. The first application uses field-free aligned molecules as a non-linear medium for compression of a laser pulse to the 1 fs regime at optical wavelengths. At such durations, these laser pulses contain nearly a single oscillation of the electric field and represent the shortest laser pulses physically achievable for such frequencies. The second application uses molecular alignment to create a sort of gas phase "molecular crystal" which forms a basis for laser-induced electron diffraction and imaging of the aligned molecules. Here, a first laser pulse aligns the molecules in space. A second laser pulse is then used to ionize outer-shell electrons, accelerate them in the laser field, and steer them back to collide with the parent ion creating a diffraction image with sub-femtosecond and sub-Angstrom resolution.

Optical cell manipulation allows precise and non-invasive exploration of mammalian cell function and physiology for medical applications. Plants, however, represent a vital component of the Earth's ecosystem and the knowledge gained from using optical tools to study plant cells can help to understand and manipulate useful agricultural and ecological traits. This thesis explores the potential of several biophotonic techniques in plant cells and tissue. Laser-mediated introduction of nucleic acids and other membrane impermeable molecules into mammalian cells is an important biophotonic technique. Optical injection presents a tool to deliver dyes and drugs for diagnostics and therapy of single cells in a sterile and interactive manner. Using femtosecond laser pulses increases the tunability of multiphoton effects and confines the damage volume, providing sub-cellular precision and high viability. Extending current femtosecond photoporation knowledge to plant cells could have sociological and environmental benefits, but presents different challenges to mammalian cells. The effects of varying optical and biological parameters on optical injection of a model plant cell line were investigated. A reconfigurable optical system was designed to allow easy switching between different spatial modes and pulse durations. Varying the medium osmolarity and optoinjectant size and type affected optoinjection efficacy, allowing optimisation of optical delivery of relevant biomolecules into plant cells. Advanced optical microscopy techniques that allow imaging beyond the diffraction limit have transformed biological studies. An ultimate goal is to merge several biophotonic techniques, creating a plant cell workstation. A step towards this was demonstrated by incorporating a fibre-based optical trap into a commercial super-resolution microscope for manipulation of cells and organelles under super-resolution. As proof-of-concept, the system was used to optically induce and quantify an immunosynapse. The capacity of the super-resolution microscope to resolve structure in plant organelles in aberrating plant tissue was critically evaluated.